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Cirrus cloud formation and evolution are subject to the influences of thermodynamic and dynamic conditions and aerosol indirect effects (AIEs). This study developed near global-scale in-situ aircraft observational datasets based on 12 field campaigns that spanned from the polar regions to the tropics, from 2008 to 2016. Cirrus cloud microphysical properties were investigated at temperatures ≤ ‑40 °C, including ice water content (IWC), ice crystal number concentration (Ni), and number-weighted mean diameter (Di). Positive correlations between the fluctuations of ice microphysical properties and the fluctuations of aerosol number concentrations for larger (> 500 nm) and smaller (> 100 nm) aerosols (i.e., Na500 and Na100, respectively) were found, with stronger AIE from larger aerosols than smaller ones. Machine learning (ML) models showed that using relative humidity with respect to ice (RHi) as a predictor significantly increases the accuracy of predicting cirrus occurrences compared with temperature, vertical velocity (w), and aerosol number concentrations. The ML predictions of IWC fluctuations showed higher accuracies when larger aerosols were used as an predictor compared with smaller aerosols, indicating the stronger AIE from larger aerosols than smaller ones, even though their AIEs are more similar when predicting the occurrences of cirrus. It is also important to capture the spatial variabilities of large aerosols at smaller scales as well as those of smaller aerosols at coarser scales to accurately simulate IWC in cirrus. These results can be used to improve understanding of aerosol-cloud interactions and evaluate model parameterizations of cirrus cloud properties and processes. 

Abstract. Sea spray aerosols (SSAs) represent one of the most abundant aerosol types on a global scale and have been observed at all altitudes including the upper troposphere. SSA has been explored in recent years as a source of ice-nucleating particles (INPs) in cirrus clouds due to the ubiquity of cirrus clouds and the uncertainties in their radiative forcing. This study expands upon previous works on low-temperature ice nucleation of SSA by investigating the effects of atmospheric aging of SSA and the ice-nucleating activity of newly formed secondary marine aerosols (SMAs) using an oxidation flow reactor. Polydisperse aerosol distributions were generated from a marine aerosol reference tank (MART) filled with 120 L of real or artificial seawater and were dried to very low relative humidity to crystallize the salt constituents of SSA prior to their subsequent freezing, which was measured using a continuous flow diffusion chamber (CFDC). Results show that for primary SSA (pSSA), as well as aged SSA and SMA (aSSA+SMA) at temperatures >220 K, homogeneous conditions (92 %–97 % relative humidity with respect to water – RHw) were required to freeze 1 % of the particles. However, below 220 K, heterogeneous nucleation occurs for both pSSA and aSSA+SMA at much lower RHw, where up to 1 % of the aerosol population freezes between 75 % and 80 % RHw. Similarities between freezing behaviors of the pSSA and aSSA+SMA at all temperatures suggest that the contributions of condensed organics onto the pSSA or alteration of functional groups in pSSA via atmospheric aging did not hinder the major heterogeneous ice nucleation process at these cirrus temperatures, which have previously been shown to be dominated by the crystalline salts. Occurrence of a 1 % frozen fraction of SMA, generated in the absence of primary SSA, was observed at or near water saturation below 220 K, suggesting it is not an effective INP at cirrus temperatures, similar to findings in the literature on other organic aerosols. Thus, any SMA coatings on the pSSA would only decrease the ice nucleation behavior of pSSA if the organic components were able to significantly delay water uptake of the inorganic salts, and apparently this was not the case. Results from this study demonstrate the ability of lofted primary sea spray particles to remain an effective ice nucleator at cirrus temperatures, even after atmospheric aging has occurred over a period of days in the marine boundary layer prior to lofting. We were not able to address aging processes under upper-tropospheric conditions. 

Abstract. Aerosols affect cirrus formation and evolution, yet quantificationof these effects remain difficult based on in situ observations due to thecomplexity of nucleation mechanisms and large variabilities in icemicrophysical properties. This work employed a method to distinguish fiveevolution phases of cirrus clouds based on in situ aircraft-basedobservations from seven U.S. National Science Foundation (NSF) and five NASAflight campaigns. Both homogeneous and heterogeneous nucleation werecaptured in the 1 Hz aircraft observations, inferred from the distributionsof relative humidity in the nucleation phase. Using linear regressions toquantify the correlations between cirrus microphysical properties andaerosol number concentrations, we found that ice water content (IWC) and icecrystal number concentration (Ni) show strong positive correlations withlarger aerosols (>500 nm) in the nucleation phase, indicatingstrong contributions of heterogeneous nucleation when ice crystals firststart to nucleate. For the later growth phase, IWC and Ni show similarpositive correlations with larger and smaller (i.e., >100 nm)aerosols, possibly due to fewer remaining ice-nucleating particles in thelater growth phase that allows more homogeneous nucleation to occur. Both200 m and 100 km observations were compared with the nudged simulations fromthe National Center for Atmospheric Research (NCAR) Community AtmosphereModel version 6 (CAM6). Simulated aerosol indirect effects are weaker thanthe observations for both larger and smaller aerosols for in situ cirrus,while the simulated aerosol indirect effects are closer to observations inconvective cirrus. The results also indicate that simulations overestimatehomogeneous freezing, underestimate heterogeneous nucleation andunderestimate the continuous formation and growth of ice crystals as cirrusclouds evolve. Observations show positive correlations of IWC, Ni and icecrystal mean diameter (Di) with respect to Na in both the Northern and SouthernHemisphere (NH and SH), while the simulations show negative correlations inthe SH. The observations also show higher increases of IWC and Ni in the SHunder the same increase of Na than those shown in the NH, indicating highersensitivity of cirrus microphysical properties to increases of Na in the SHthan the NH. The simulations underestimate IWC by a factor of 3–30 in theearly/later growth phase, indicating that the low bias of simulated IWC wasdue to insufficient continuous ice particle formation and growth. Sucha hypothesis is consistent with the model biases of lower frequencies of icesupersaturation and lower vertical velocity standard deviation in theearly/later growth phases. Overall, these findings show that aircraftobservations can capture both heterogeneous and homogeneous nucleation, andtheir contributions vary as cirrus clouds evolve. Future model developmentis also recommended to evaluate and improve the representation of watervapor and vertical velocity on the sub-grid scale to resolve theinsufficient ice particle formation and growth after the initial nucleationevent. 

Aerosols affect cirrus formation and evolution, yet quantification of these effects remain difficult based on in-situ observations due to the complexity of nucleation mechanisms and large variabilities in ice microphysical properties. This work employed a method to distinguish five evolution phases of cirrus clouds based on in-situ aircraft-based observations from seven U.S. National Science Foundation (NSF) and five NASA flight campaigns. Both homogeneous and heterogeneous nucleation were captured in the 1-Hz aircraft observations, inferred from the distributions of relative humidity in the nucleation phase. Using linear regressions to quantify the correlations between cirrus microphysical properties and aerosol number concentrations, we found that ice water content (IWC) and ice crystal number concentration (Ni) show strong positive correlations with larger aerosols (> 500 nm) in the nucleation phase, indicating strong contributions of heterogeneous nucleation when ice crystals first start to nucleate. For the later growth phase, IWC and Ni show similar positive correlations with larger and smaller (i.e., > 100 nm) aerosols, possibly due to fewer remaining ice nucleating particles in the later growth phase that allows more homogeneous nucleation to occur. Both 200-m and 100-km observations were compared with the nudged simulations from the National Center for Atmospheric Research (NCAR) Community Atmosphere Model version 6 (CAM6). Simulated aerosol indirect effects are weaker than the observations for both larger and smaller aerosols. Observations show stronger aerosol indirect effects (i.e., positive correlations between IWC, Ni and Na) in the Southern Hemisphere (SH) compared with the Northern Hemisphere (NH), while the simulations show negative correlations in the SH. The simulations underestimate IWC by a factor of 3 – 30 in the early/later growth phase, indicating that the low bias of simulated IWC was due to insufficient ice particle growth. Such hypothesis is consistent with the model biases of lower frequencies of ice supersaturation and lower vertical velocity standard deviation in the early/later growth phases. Overall, these findings show that aircraft observations can capture the competitions between heterogeneous and homogeneous nucleation, and their contributions vary as cirrus clouds evolve. Future model development is also recommended to evaluate and improve the representation of water vapor and vertical velocity on the sub-grid scale to resolve the insufficient ice particle growth. 

Abstract The secondary ice process (SIP) is a major microphysical process, which can result in rapid enhancement of ice particle concentration in the presence of preexisting ice. SPICULE was conducted to further investigate the effect of collision–coalescence on the rate of the fragmentation of freezing drop (FFD) SIP mechanism in cumulus congestus clouds. Measurements were conducted over the Great Plains and central United States from two coordinated aircraft, the NSF Gulfstream V (GV) and SPEC Learjet 35A, both equipped with state-of-the-art microphysical instrumentation and vertically pointing W- and Ka-band radars, respectively. The GV primarily targeted measurements of subcloud aerosols with subsequent sampling in warm cloud. Simultaneously, the Learjet performed multiple penetrations of the ascending cumulus congestus (CuCg) cloud top. First primary ice was typically detected at temperatures colder than −10°C, consistent with measured ice nucleating particles. Subsequent production of ice via FFD SIP was strongly related to the concentration of supercooled large drops (SLDs), with diameters from about 0.2 to a few millimeters. The concentration of SLDs is directly linked to the rate of collision–coalescence, which depends primarily on the subcloud aerosol size distribution and cloud-base temperature. SPICULE supports previous observational results showing that FFD SIP efficiency could be deduced from the product of cloud-base temperature and maximum diameter of drops measured ∼300 m above cloud base. However, new measurements with higher concentrations of aerosol and total cloud-base drop concentrations show an attenuating effect on the rate of coalescence. The SPICULE dataset provides rich material for validation of numerical schemes of collision–coalescence and SIP to improve weather prediction simulations 

Abstract Convective clouds play an important role in the Earth’s climate system and are a known source of extreme weather. Gaps in our understanding of convective vertical motions, microphysics, and precipitation across a full range of aerosol and meteorological regimes continue to limit our ability to predict the occurrence and intensity of these cloud systems. Towards improving predictability, the National Science Foundation (NSF) sponsored a large field experiment entitled “Experiment of Sea Breeze Convection, Aerosols, Precipitation, and Environment (ESCAPE).” ESCAPE took place between 30 May - 30 Sept. 2022 in the vicinity of Houston, TX because this area frequently experiences isolated deep convection that interacts with the region's mesoscale circulations and its range of aerosol conditions. ESCAPE focused on collecting observations of isolated deep convection through innovative sampling, and on developing novel analysis techniques. This included the deployment of two research aircraft, the National Research Council of Canada Convair-580 and the Stratton Park Engineering Company Learjet, which combined conducted 24 research flights from 30 May to 17 June. On the ground, three mobile X-band radars, and one mobile Doppler lidar truck equipped with soundings, were deployed from 30 May to 28 June. From 1 August to 30 Sept. 2022, a dual-polarization C-band radar was deployed and operated using a novel, multi-sensor agile adaptive sampling strategy to track the entire lifecycle of isolated convective clouds. Analysis of the ESCAPE observations has already yielded preliminary findings on how aerosols and environmental conditions impact the convective life cycle. 

Abstract. Cirrus cloud radiative effects are largely affected byice microphysical properties, including ice water content (IWC), ice crystalnumber concentration (Ni) and mean diameter (Di). These characteristics varysignificantly due to thermodynamic, dynamical and aerosol conditions. Inthis work, a global-scale observation dataset is used to examine regionalvariations of cirrus cloud microphysical properties, as well as several keycontrolling factors, i.e., temperature, relative humidity with respect toice (RHi), vertical velocity (w) and aerosol number concentrations (Na).Results are compared with simulations from the National Center forAtmospheric Research (NCAR) Community Atmosphere Model version 6 (CAM6).Observed and simulated ice mass and number concentrations are constrained to≥62.5 µm to reduce potential uncertainty from shattered ice indata collection. The differences between simulations and observations arefound to vary with latitude and temperature. Comparing with averagedobservations at ∼100 km horizontal scale, simulations arefound to underestimate (overestimate) IWC by a factor of 3–10 in theNorthern (Southern) Hemisphere. Simulated Ni is overestimated in mostregions except the Northern Hemisphere midlatitudes. Simulated Di isunderestimated by a factor of 2, especially for warmer conditions(−50 to −40 ∘C), possibly due tomisrepresentation of ice particle growth/sedimentation. For RHi effects, thefrequency and magnitude of ice supersaturation are underestimated insimulations for clear-sky conditions. The simulated IWC and Ni show bimodaldistributions with maximum values at 100 % and 80 % RHi, differing fromthe unimodal distributions that peak at 100 % in the observations. For weffects, both observations and simulations show variances of w (σw) decreasing from the tropics to polar regions, but simulations show muchhigher σw for the in-cloud condition than the clear-sky condition.Compared with observations, simulations show weaker aerosol indirect effectswith a smaller increase of IWC and Di at higher Na. These findings provide anobservation-based guideline for improving simulated ice microphysicalproperties and their relationships with key controlling factors at variousgeographical locations. 

Cirrus cloud radiative effects are largely affected by ice microphysical properties, including ice water content (IWC), ice crystal number concentration (Ni) and mean diameter (Di). These characteristics vary significantly due to thermodynamic, dynamical and aerosol conditions. In this work, a global-scale observation dataset is used to examine regional variations of cirrus cloud microphysical properties, as well as several key controlling factors, i.e., temperature, relative humidity with respect to ice (RHi), vertical velocity (w), and aerosol number concentrations (Na). Results are compared with simulations from the National Center for Atmospheric Research (NCAR) Community Atmosphere Model version 6 (CAM6). The differences between simulations and observations are found to vary with latitude and temperature. Specifically, simulations are found to underestimate IWC by a factor of 5–30 in all regions. Simulated Ni is overestimated in most regions except Northern Hemisphere midlatitude and polar regions. Simulated Di is underestimated, especially for warmer conditions (−50 °C to −40 °C) and higher Na, possibly due to less effective ice particle growth/sedimentation and weaker aerosol indirect effects, respectively. For RHi effects, the frequency and magnitude of ice supersaturation is underestimated in simulations for clear-sky conditions, and the simulated IWC and Ni show maximum values at 80 % RHi instead of 110 % as observed. For w effects, both observations and simulations show variances of w (σw) decreasing from tropics to polar regions, but simulations show much higher σw for in-cloud condition than clear-sky condition. These findings provide an observation-based guideline for improving simulated ice microphysical properties and their relationships with key controlling factors at various geographical locations.